CN114985446A - Method for synchronously reducing cadmium and arsenic content of rice in acidic cadmium-arsenic composite polluted rice field - Google Patents
Method for synchronously reducing cadmium and arsenic content of rice in acidic cadmium-arsenic composite polluted rice field Download PDFInfo
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C1/00—Reclamation of contaminated soil
- B09C1/08—Reclamation of contaminated soil chemically
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- A—HUMAN NECESSITIES
- A01—AGRICULTURE; FORESTRY; ANIMAL HUSBANDRY; HUNTING; TRAPPING; FISHING
- A01B—SOIL WORKING IN AGRICULTURE OR FORESTRY; PARTS, DETAILS, OR ACCESSORIES OF AGRICULTURAL MACHINES OR IMPLEMENTS, IN GENERAL
- A01B79/00—Methods for working soil
- A01B79/02—Methods for working soil combined with other agricultural processing, e.g. fertilising, planting
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- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K17/00—Soil-conditioning materials or soil-stabilising materials
- C09K17/02—Soil-conditioning materials or soil-stabilising materials containing inorganic compounds only
- C09K17/06—Calcium compounds, e.g. lime
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C2101/00—In situ
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
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- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K2109/00—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE pH regulation
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Abstract
The invention provides a method for synchronously reducing the content of cadmium and arsenic in rice of acid cadmium and arsenic composite polluted rice fields. According to the method, under the condition of continuous flooding, a sufficient amount of calcium-based pH regulator is applied to the soil until the soil is alkalescent (the pH is 7.0-7.5), and a proper amount of magnetite and soluble sulfide are applied in a combined manner, so that the effects of relieving the toxicity of Cd and As to rice and remarkably reducing the Cd and As content of grains are achieved, and particularly the As content in rice grains is remarkably reduced. The applied raw materials are low in cost, the application method is simple, the effect is obvious, and the large-scale popularization is easy.
Description
Technical Field
The invention relates to the technical field of soil pollution remediation, in particular to a method for synchronously reducing the content of cadmium and arsenic in rice of an acid cadmium-arsenic composite polluted rice field.
Background
Due to the mining of metal mines, the discharge of industrial wastes, the application of cadmium/arsenic (Cd/As) containing pesticides, chemical fertilizers and organic fertilizers in large quantities, Cd and As compound pollution exists in the rice field. According to the national soil pollution condition survey bulletin published in 2014 of the ministry of environmental protection and the ministry of homeland, the exceeding rate of Cd point position in cultivated land of China reaches 7.0 percent, the exceeding rate of As reaches 2.7 percent, and the first and third place pollution elements are discharged. Compared with other elements, Cd and As are elements which are easier to be absorbed by rice and transported to rice grains. The rice is a main food crop in China, health risks can be caused even if Cd and As are taken in for a long time at low dose, and the reduction of the cadmium and arsenic content in the rice produced by the Cd and As polluted rice fields is a major environmental and food safety problem related to the health of people and the sustainable development of agriculture.
The remediation of cadmium and arsenic composite pollution of the rice field is a difficult problem in the environmental field. Cadmium and arsenic have different chemical properties, and the lower oxidation-reduction potential is helpful for reducing the plant absorption of cadmium, but the toxicity is increased due to arsenic reduction. Higher pH is beneficial for stabilizing Cd but increases the solubility of As. The activity of Cd and As is difficult to be regulated and controlled simultaneously by regulating the pH value and the oxidation-reduction potential (Eh) of soil, which brings difficulties and challenges to the remediation of the soil polluted by Cd and As in the rice field and the safe production of rice. The current technical means for treating the cadmium-arsenic composite pollution of soil is relatively lacking. The main repair methods at present comprise (1) super-accumulation plant extraction: plants which accumulate excessive cadmium or arsenic are used for absorbing cadmium and arsenic, and the cadmium and arsenic content of the soil is reduced by harvesting the plants, but the method has the problems of long repair period, farmland occupation, high cost and the like for the moderately and heavily polluted soil. (2) Soil passivation and remediation: materials such as iron-manganese base materials, biochar materials and clay minerals: although the method has a certain fixing effect on cadmium and arsenic, the method has high cost and has the risk of secondary re-release of cadmium and arsenic. (3) Leaf surface regulation and control: exogenous silicon (Si), selenium (Se), zinc (Zn) and the like are sprayed on the leaf surfaces to control cadmium or arsenic in rice, the dosage is small, the cost is low, attention is paid to the conditioner, the conditioner mainly aims at single heavy metal, meanwhile, the leaf surface conditioner also has the problems of unstable effect and urgent need for improvement of the repair efficiency.
Although some researchers have studied methods for simultaneously reducing the content of cadmium and arsenic in soil and rice, for example, the idea of synchronously repairing cadmium and arsenic fixed by sodium thiosulfate in situ extraction and zero-valent iron adsorption in Chinese patent CN110144224A is adopted, sodium thiosulfate used therein is easily oxidized by oxygen in the air to generate sulfur dioxide, and the sulfur dioxide is easily absorbed by the wet mucosa surface to generate sulfurous acid and sulfuric acid, so that the method has strong stimulation effect on the eyes and respiratory mucosa; there are also studies (for example, Chinese patent CN112845564A) on the use of soluble sulfides (e.g., K) 2 S) and a calcium-based pH regulator (such As calcium carbonate) are applied together to reduce the content of cadmium and arsenic in soil, but because the pollution degree of As element in the actually polluted soil is far higher than that of Cd element, the regulator has weak inhibition on the As element.
Therefore, a new method for synchronously reducing the cadmium and arsenic content of the rice in the acid cadmium-arsenic composite polluted rice field with low cost, simple application, stability and high efficiency (especially for inhibiting As) is needed to be developed aiming at the acid cadmium-arsenic composite polluted rice field with high As content.
Disclosure of Invention
Based on the above, the invention aims to overcome the defect that the existing soil cadmium arsenic remediation regulator has poor inhibition effect on As, and provides a novel method which is low in cost, simple to apply, stable and efficient (especially efficient inhibition on As) and can synchronously reduce the content of cadmium and arsenic in the acidic cadmium-arsenic composite polluted rice field. The invention can safely and synchronously reduce the cadmium and arsenic content of the rice with low cost, thereby achieving the aim of safe production.
In order to realize the purpose, the invention adopts the following technical scheme:
a method for synchronously reducing the content of cadmium and arsenic in rice of acidic cadmium and arsenic composite polluted rice fields comprises the following steps:
s1, covering a water layer on the soil surface of the acid cadmium arsenic compound polluted paddy field with a thickness of more than or equal to 4cm before planting paddy rice, and keeping the soil surface flooded in the whole growth period of the paddy rice until harvesting;
s2, adding a calcium-based pH regulator into the flooded soil obtained in the S1 to regulate the pH of the soil to 7.0-7.5;
s3, adding magnetite and soluble sulfide into the soil obtained in the S2, and uniformly mixing;
wherein the molar content of calcium in the calcium-based pH regulator is greater than the total molar content of arsenic in the soil; the total molar quantity of calcium element and sulfur element in soluble sulfide in the calcium-based pH regulator is more than or equal to the total molar quantity of cadmium and arsenic in soil; the molar ratio of the sulfur element in the soluble sulfide to the total content of cadmium and arsenic in the acid cadmium and arsenic compositely polluted paddy soil is (5-25): 1; the addition amount of the magnetite is 0.1-5.0% of the weight of the soil.
According to the invention, sufficient alkaline calcium-based pH regulator, a proper amount of magnetite and soluble sulfide are jointly applied under the continuous flooding condition of the acidic paddy soil, so that the aim of obviously reducing the content of Cd and As in the brown rice is achieved. In the invention, on one hand, the alkaline calcium-based pH regulator improves the pH of the soil to be about neutral and reduces the cadmium activity of the soil; on the other hand, the method can also have precipitation reaction with Cd and As, thereby obviously reducing the activity of Cd and As in soil and reducing the absorption of rice. In addition, under the conditions of neutral or alkalescent pH and continuous flooding, magnetite and soluble sulfide interact, secondary iron oxide and iron-sulfur minerals with high adsorption activity are easily promoted and strengthened to be formed, an iron film on the surface of the root of the rice is promoted to be formed, and active Cd and As can be strongly adsorbed to inhibit the Cd and As from entering the body of the rice. The added sulfur enters the rice body, the synthesis of Glutathione (GSH) and Phytochelatin (PCs) in the rice body can be promoted, Cd and As chelated and entering the plant body are transferred to rice root, stem and leaf cell vacuoles for separation, and the Cd and As are fixed at corresponding positions, so that the transfer and accumulation of the Cd and As entering the rice body to grains are reduced. Finally, the aim of synchronously reducing the content of cadmium and arsenic in the brown rice is achieved, and particularly, the content of As in soil and rice is obviously reduced.
The addition amount of magnetite is too much, which can cause the yield reduction of grains; the addition amount is too small, the cadmium arsenic activity of soil cannot be obviously inhibited, and the reduction of the content of Cd and As in rice grains is not facilitated. Further preferably, the magnetite is added in an amount of 0.5% by weight of the soil.
Preferably, the calcium isThe pH regulator is at least one of calcium carbonate, dolomite, calcium oxide or calcium hydroxide. More preferably calcium carbonate (CaCO) 3 ) Because of CaCO 3 Can simultaneously generate precipitation reaction with Cd and As to form cadmium carbonate (CdCO) 3 )、Cd(OH) 2 Calcium arsenate (CaAsO) 4 ) Thereby obviously reducing the activity of Cd and As in soil and reducing the absorption of rice.
The soil surface of the acid paddy field is covered with a water layer, so that the soil environment can be kept in a reduction environment, the interaction between magnetite and soluble sulfide is facilitated, the formation of secondary iron oxide and iron-sulfur minerals with high adsorption activity is promoted, and the formation of an iron film on the surface of the root of the paddy rice is promoted, so that the soil active Cd and As are strongly adsorbed, and the soil active state Cd and As are inhibited from entering the paddy rice body.
Preferably, the soluble sulfide is K 2 S or Na 2 At least one of S; further preferably K 2 S。
Elemental sulfur (S) in suitable soluble sulfides 2- ) The application amount of the fertilizer is beneficial to reducing the content of active cadmium and arsenic in soil, and simultaneously, the fertilizer does not generate toxic action on plants. S 2- Too much, the soil can be acidified, and the plant can be poisoned; s. the 2- If the amount of the cadmium and the arsenic in the soil is too small, the reduction of the content of the cadmium and the arsenic in the soil is not obvious, and the effect of restoring the cadmium and arsenic combined pollution of the acid paddy soil can not be achieved. Further preferably, in the step s3, the molar ratio of the sulfur element in the soluble sulfide to the total content of cadmium and arsenic in the acidic cadmium and arsenic compositely polluted paddy soil is (10-15): 1.
preferably, the pH value of the acidic cadmium arsenic compound polluted paddy soil is 3-6.5.
Preferably, the content of Cd in the acidic cadmium arsenic compound polluted paddy soil is 0.1-2.0 mg/kg.
Preferably, the content of As in the acidic cadmium arsenic compound polluted paddy soil is 10-120 mg/kg.
Compared with the prior art, the invention has the beneficial effects that:
according to the method, under the condition of continuous flooding, a sufficient amount of calcium-based pH regulator is applied to the soil until the soil is alkalescent (the pH is 7.0-7.5), and a proper amount of magnetite and soluble sulfide are applied in a combined manner, so that the effects of relieving the toxicity of Cd and As to rice and reducing the Cd and As content of grains are achieved, and particularly the As content in rice grains is remarkably reduced. The applied raw materials are low in cost, the application method is simple, the effect is obvious, and the large-scale popularization is easy.
Detailed Description
The present invention will be further described with reference to specific examples for better illustrating the objects, technical solutions and advantages of the present invention, but the examples are not intended to limit the present invention in any way. Reagents, methods and apparatus used in the present invention are conventional in the art unless otherwise indicated. Unless otherwise indicated, reagents and materials used in the present invention are commercially available.
The acid cadmium-arsenic composite polluted rice field soil used in the following examples and comparative examples is collected from a cadmium-arsenic composite polluted rice field at the downstream of a certain mining area in Guangdong province, the pH value of the soil is 4.5, the total Cd content of the soil is 1.0mg/kg, and the total As content of the soil is 80.0 mg/kg.
Heavy metal content in the raw materials (including calcium-based pH adjusting agent, magnetite, and soluble sulfide) applied in examples and comparative examples: cd is less than or equal to 1.0mg/kg, Pb is less than or equal to 100mg/kg, Cr is less than or equal to 150mg/kg, As is less than or equal to 30mg/kg, and Hg is less than or equal to 2.0 mg/kg.
Example 1
The embodiment provides a method for synchronously reducing the content of cadmium and arsenic in rice of an acidic cadmium-arsenic composite polluted rice field, which comprises the following steps:
s1, drying the collected acidic cadmium arsenic composite polluted paddy soil in air, sieving the soil with a 10-mesh sieve, and taking 4kg of sieved soil (the Cd content in the soil is 8.8968 multiplied by 10) -6 Filling the soil with mol/kg, the As content of 0.0010678mol/kg and the total content of Cd and As of 0.0010767mol/kg into a plastic pot (the height is 30cm, the caliber is 25cm), applying 1.8g of NPK compound fertilizer As a base fertilizer in the pot, and watering until the surface of the soil can keep a 4-5 cm water layer;
s2, adding calcium carbonate (sieved by a 20-mesh sieve) into the soil obtained in the step S1 until the pH value of the soil is 7.0-7.5 (as the pH value of the soil is buffered, the content of components in different parts of the soil possibly differs, and the specific values of the pH values possibly differ at different sampling parts, the pH value of each part of the soil is ensured to be within the range of 7.0-7.5);
s3, adding 0.01247mol/kg of soil (1.3775g K) with S content into the soil obtained in the step S2 2 S/kg soil) K 2 S, 20g of magnetite (namely 0.5 percent of the weight of the soil), and fully and uniformly mixing;
balancing the acidic cadmium-arsenic compound contaminated paddy field soil obtained after the treatment in the step S3 for 2 weeks under the condition that a water layer on the surface of the soil is kept at 4-6 cm, and then transplanting rice seedlings (25 days old); wherein, three groups of the seedlings are arranged repeatedly, 2 holes are arranged in each pot, and 3 seedlings are arranged in each hole. And keeping the soil surface flooded by 4-5 cm by pure water in the whole growth period of the rice until harvesting.
Example 2
The embodiment provides a method for synchronously reducing the content of cadmium and arsenic in rice in an acidic cadmium-arsenic composite polluted rice field, which is different from the embodiment 1 in that: the amount of magnetite added was 4g magnetite (i.e. 0.1% of the soil weight).
Example 3
The embodiment provides a method for synchronously reducing cadmium and arsenic content in rice of acidic cadmium-arsenic composite polluted rice field, which is different from the embodiment 1 in that: the amount of magnetite added was 200g magnetite (i.e. 5% of the soil weight).
Example 4
The embodiment provides a method for synchronously reducing the content of cadmium and arsenic in rice in an acidic cadmium-arsenic composite polluted rice field, which is different from the embodiment 1 in that: step S3. adding K 2 Replacement of S by Na 2 S。
Comparative example 1
This comparative example is different from example 1 in that calcium carbonate, magnetite and K were not added 2 S, is denoted as blank processing (CK).
Comparative example 2
The comparative example provides a method for reducing the content of cadmium and arsenic in rice in acidic cadmium-arsenic composite polluted rice field, and compared with example 1, the difference is that K is not added 2 S。
Comparative example 3
Compared with the example 1, the difference of the method for reducing the content of cadmium and arsenic in the rice of the acid cadmium-arsenic composite polluted rice field is that magnetite is not added.
Comparative example 4
The comparative example provides a method for reducing the content of cadmium and arsenic in rice in acidic cadmium-arsenic composite polluted rice field, and compared with example 1, the difference is that K is 2 S is replaced by K 2 SO 4 。
Test results
The rice of the above examples and comparative examples was grown and harvested four months later, and rice plant seeds and soil were collected. Putting the rice grains in a drying oven, deactivating enzymes at 105 ℃ for 30 minutes, drying at 70 ℃ until the weight is kept stable, measuring the yield (g/plant), then putting the rice grains in a stainless steel grinding machine for crushing and grinding, and sieving by a 100-mesh sieve; the soil sample is directly air-dried in the air, ground, uniformly mixed and sieved by a 100-mesh sieve for later use.
Determining the cadmium and arsenic content in rice grains and soil:
1. cadmium and arsenic in the rice grains are digested and the content of the cadmium and the arsenic is measured: weighing 1g of the ground seed sample, adding 9mL of concentrated nitric acid and 4mL of hydrogen peroxide, and standing for 12 hours; then, the sample is further subjected to microwave digestion treatment (180 ℃, 30 minutes), and after cooling and dilution, the concentration of total arsenic and total cadmium in the solution is analyzed and measured on an inductively coupled plasma mass spectrometer (ICP-OES) and a graphite furnace atomic absorption spectrometer. Wherein, three groups of repeated experiments of each treatment are respectively measured, and the average value of the three groups of repeated experiments is taken as a test result, and the test result is detailed in table 1;
wherein, the rice yield increase rate (%) ═ yield of each example or comparative example-yield of comparative example 1 (CK)/[ yield of comparative example 1(CK) ] is 100%;
percent (%) reduction of Cd in rice ═ Cd content of comparative example 1(CK) — Cd content of each example or comparative example/[ Cd content of comparative example 1(CK) ] 100%;
as reduction rate (%) in rice ═ As content of comparative example 1(CK) — As content of each example or comparative example/[ As content of comparative example 1(CK) ] 100%;
2. extracting cadmium and arsenic in soil and measuring the content of cadmium and arsenic: 2.0000g of soil sample was added to a 50mL centrifuge tube, followed by 20mL of 0.01M CaCl 2 Shaking the solution at 20 deg.C for 6h, centrifuging at 4000g for 10min, collecting supernatant, digesting, filtering, measuring arsenic with ICP-OES, and measuring cadmium with graphite furnace atomic absorption. Wherein, three groups of repeated experiments of each treatment are respectively measured, the average value of the three groups of repeated experiments is taken as a test result, the test result is detailed in table 1, and the reduction rate of cadmium and arsenic in soil is the same as the calculation mode in rice.
TABLE 1 test results
The results in table 1 show that:
under the condition of continuous flooding, sufficient calcium-based pH regulator is applied to the soil to be neutral-alkalescent (the pH is 7.0-7.5), and a proper amount of magnetite and soluble sulfide are applied in combination, so that the effects of relieving the toxicity of Cd and As to rice and remarkably reducing the content of Cd and As in grains can be achieved. Wherein, compared with blank processing (CK), the yield of rice can be improved by as high as 101%; the content of Cd in the rice can be reduced to 21%; the content of As in the rice can be reduced by 76 percent, so that the combination of the regulator has obvious effect on reducing the content of Cd and As in the rice. Other examples have a simultaneous reduction effect on Cd and As in rice, but the effect is inferior to that of example 1.
The results of the embodiment and the comparative examples 2-5 show that the soluble sulfide and the magnetite jointly reduce the absorption of Cd and As by the rice through multi-directional synergistic effect, and particularly the content of As in the rice is obviously reduced.
Finally, it should be noted that the above embodiments are only used for illustrating the technical solutions of the present invention and not for limiting the protection scope of the present invention, and although the present invention is described in detail with reference to the preferred embodiments, it should be understood by those skilled in the art that modifications or equivalent substitutions can be made on the technical solutions of the present invention without departing from the spirit and scope of the technical solutions of the present invention.
Claims (9)
1. A method for synchronously reducing the content of cadmium and arsenic in rice of acidic cadmium and arsenic composite polluted rice is characterized by comprising the following steps:
s1, covering a water layer on the soil surface of the acid cadmium arsenic compound polluted paddy field with a thickness of more than or equal to 4cm before planting paddy rice, and keeping the soil surface flooded in the whole growth period of the paddy rice until harvesting;
s2, adding a calcium-based pH regulator into the flooded soil obtained in the S1 to regulate the pH of the soil to 7.0-7.5;
s3, adding magnetite and soluble sulfide into the soil obtained in the S2, and uniformly mixing;
wherein the molar content of calcium in the calcium-based pH regulator is greater than the total molar content of arsenic in the soil; the total molar quantity of calcium element and sulfur element in soluble sulfide in the calcium-based pH regulator is more than or equal to the total molar quantity of cadmium and arsenic in soil; the molar ratio of the sulfur element in the soluble sulfide to the total content of cadmium and arsenic in the acid cadmium and arsenic compositely polluted paddy soil is (5-25): 1; the addition amount of the magnetite is 0.1-3.0% of the weight of the soil.
2. The method for synchronously reducing the cadmium and arsenic content in the rice of the acid cadmium-arsenic composite polluted rice field as claimed in claim 1, wherein the addition amount of the magnetite is 0.5 percent of the weight of the soil.
3. The method for synchronously reducing the cadmium and arsenic content in the rice in the acidic cadmium-arsenic co-polluted rice field as claimed in claim 1, wherein the calcium-based pH regulator is at least one of calcium carbonate, dolomite, calcium oxide or calcium hydroxide.
4. The method for synchronously reducing the cadmium and arsenic content in the rice in the acidic cadmium-arsenic co-polluted rice field as claimed in claim 1, wherein the calcium-based pH regulator is calcium carbonate.
5. The sync reduction of claim 1The method for the cadmium and arsenic content of the rice of the acidic cadmium-arsenic compound polluted rice field is characterized in that the soluble sulfide is K 2 S or Na 2 At least one of S.
6. The method for synchronously reducing the cadmium and arsenic content in the rice in the acidic cadmium-arsenic compound contaminated rice field as claimed in claim 1, wherein in the step s3, the molar ratio of the sulfur element in the soluble sulfide to the total cadmium and arsenic content in the acidic cadmium-arsenic compound contaminated rice field soil is (10-15): 1.
7. the method for synchronously reducing the content of cadmium and arsenic in rice in the acidic cadmium-arsenic co-polluted rice field as claimed in claim 1, wherein the pH of the acidic cadmium-arsenic co-polluted rice field soil is 3-6.5.
8. The method for synchronously reducing the cadmium and arsenic content in the rice in the acidic cadmium-arsenic co-polluted rice field as claimed in claim 1, wherein the Cd content in the acidic cadmium-arsenic co-polluted rice field soil is 0.1-2.0 mg/kg.
9. The method for synchronously reducing the cadmium and arsenic content in the rice in the acidic cadmium-arsenic co-polluted rice field As claimed in claim 1, wherein the As content in the soil in the acidic cadmium-arsenic co-polluted rice field is 10-120 mg/kg.
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